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This work presents an alternative, general, and in-principle exact extension of electronic Kohn-Sham density functional theory (KS-DFT) to the fully quantum-mechanical molecular problem. Unlike in existing multi-component or…

Chemical Physics · Physics 2024-05-14 Emmanuel Fromager , Benjamin Lasorne

We study model one-dimensional chemical systems (representative of their three-dimensional counterparts) using the strictly-correlated electrons (SCE) functional, which, by construction, becomes asymptotically exact in the limit of infinite…

The exchange-correlation energy in Kohn-Sham density functional theory can be expressed exactly in terms of the change in the expectation of the electron-electron repulsion operator when, in the many-electron hamiltonian, this same operator…

Strongly Correlated Electrons · Physics 2009-08-05 Paola Gori-Giorgi , Giovanni Vignale , Michael Seidl

We present a rigorous formulation of generalized Kohn-Sham density-functional theory. This provides a straightforward Kohn-Sham description of many-body systems based not only on particle-density but also on any other observable. We…

Strongly Correlated Electrons · Physics 2008-02-03 M. Valiev , G. W. Fernando

The exchange-correlation hole density of the infinitely stretched (dissociated) hydrogen molecule can be cast into a closed analytical form by using its exact wave function. This permits to obtain an explicit exchange-correlation energy…

Chemical Physics · Physics 2017-11-16 Eduard Matito , David Casanova , Xabier Lopez , Jesus M. Ugalde

We propose exchanging the energy functionals in ground-state DFT with physically equivalent exact force expressions as a new promising route towards approximations to the exchange-correlation potential and energy. In analogy to the usual…

We present and test a new approximation for the exchange-correlation (xc) energy of Kohn-Sham density functional theory. It combines exact exchange with a compatible non-local correlation functional. The functional is by construction free…

Chemical Physics · Physics 2014-05-23 Tobias Schmidt , Eli Kraisler , Adi Makmal , Leeor Kronik , Stephan Kümmel

Kohn-Sham (KS) density functional theory (DFT) is a very efficient method for calculating various properties of solids as, for instance, the total energy, the electron density, or the electronic band structure. The KS-DFT method leads to…

Materials Science · Physics 2019-09-20 Fabien Tran , Jan Doumont , Leila Kalantari , Ahmad W. Huran , Miguel A. L. Marques , Peter Blaha

We propose a scheme to extract the many-body spectral function of an interacting many-electron system from an equilibrium density functional theory (DFT) calculation. To this end we devise an ideal STM-like setup and employ the recently…

Mesoscale and Nanoscale Physics · Physics 2018-02-20 David Jacob , Stefan Kurth

Practical density functional theory (DFT) owes its success to the groundbreaking work of Kohn and Sham that introduced the exact calculation of the non-interacting kinetic energy of the electrons using an auxiliary mean-field system.…

Chemical Physics · Physics 2023-11-17 P. del Mazo-Sevillano , J. Hermann

We model the Hartree-exchange-correlation potential of Kohn-Sham density-functional theory adopting a novel strategy inspired by the strictly-correlated-electrons limit and relying on the exact decomposition of the potential based on the…

Chemical Physics · Physics 2024-09-09 Sara Giarrusso , Federica Agostini

Exchange interactions are a manifestation of the quantum mechanical nature of the electrons and play a key role in predicting the properties of materials from first principles. In density functional theory (DFT), a widely used approximation…

Materials Science · Physics 2020-03-27 Marco Bernardi

Current-spin density functional theory (CSDFT) provides a framework to describe interacting many-electron systems in a magnetic field which couples to both spin- and orbital-degrees of freedom. Unlike in usual (spin-) density functional…

Materials Science · Physics 2015-06-25 S. Pittalis , S. Kurth , N. Helbig , E. K. U. Gross

We analytically construct the wave function that, for a given initial state, produces a prescribed density for a quantum ring with two non-interacting particles in a singlet state. In this case the initial state is completely determined by…

Strongly Correlated Electrons · Physics 2013-08-23 M. Ruggenthaler , S. E. B. Nielsen , R. van Leeuwen

Adsorbed transition metal atoms can have partially filled $d$- or $f$-shells due to strong on-site Coulomb interaction. Capturing all effects originating from electron correlation in such strongly correlated systems is a challenge for…

Strongly Correlated Electrons · Physics 2018-01-17 Marc Philipp Bahlke , Michael Karolak , Carmen Herrmann

The widely-used Kohn-Sham implementation of density functional theory (DFT) maps a system of interacting electrons onto an auxiliary non-interacting one and is presumably inaccurate for strongly correlated materials. We present a concrete…

Strongly Correlated Electrons · Physics 2024-05-31 Jamin Kidd , Ruiqi Zhang , Shao-Kai Jian , Jianwei Sun

We present analytic expressions for the exact density functional and Kohn-Sham Hamiltonian of simple tight-binding models of correlated electrons. These are the single- and double-site versions of the Anderson, Hubbard and spinless fermion…

Strongly Correlated Electrons · Physics 2012-01-16 D. J. Carrascal , J. Ferrer

The construction of a better exchange-correlation potential in time-dependent density functional theory (TDDFT) can improve the accuracy of TDDFT calculations and provide more accurate predictions of the properties of many-electron systems.…

Quantum Physics · Physics 2023-08-23 Jun Yang , James D Whitfield

A density functional theory (DFT) framework is presented that links functional derivatives of free-energy functionals to non-linear static density response functions in quantum many-body systems. Within this framework, explicit expressions…

The accurate description of open-shell molecules, in particular of transition metal complexes and clusters, is still an important challenge for quantum chemistry. While density-functional theory (DFT) is widely applied in this area, the…

Chemical Physics · Physics 2012-10-26 Christoph R. Jacob , Markus Reiher